H2-driven biocatalysis for flavin-dependent ene-reduction in a continuous closed-loop flow system utilizing H2 from water electrolysis
Guiyeoul Lim (RWTH Aachen University)
Donato Calabrese (RWTH Aachen University)
A.E. Wolder (TU Delft - BT/Biocatalysis)
Paul R.F. Cordero (RWTH Aachen University)
Dörte Rother (RWTH Aachen University, Forschungszentrum Jülich)
Florian F. Mulks (RWTH Aachen University)
Caroline E. Paul (TU Delft - BT/Biocatalysis)
Lars Lauterbach (RWTH Aachen University)
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Abstract
Despite the increasing demand for efficient and sustainable chemical processes, the development of scalable systems using biocatalysis for fine chemical production remains a significant challenge. We have developed a scalable flow system using immobilized enzymes to facilitate flavin-dependent biocatalysis, targeting as a proof-of-concept asymmetric alkene reduction. The system integrates a flavin-dependent Old Yellow Enzyme (OYE) and a soluble hydrogenase to enable H2-driven regeneration of the OYE cofactor FMNH2. Molecular hydrogen was produced by water electrolysis using a proton exchange membrane (PEM) electrolyzer and introduced into the flow system via a designed gas membrane addition module at a high diffusion rate. The flow system shows remarkable stability and reusability, consistently achieving >99% conversion of ketoisophorone to levodione. It also demonstrates versatility and selectivity in reducing various cyclic enones and can be extended to further flavin-based biocatalytic approaches and gas-dependent reactions. This electro-driven continuous flow system, therefore, has significant potential for advancing sustainable processes in fine chemical synthesis.
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